28-: A New Polyoxometalate Structural Family with Catalytic Hydrogen Evolution Activity

Hongjin Lv; Yingnan Chi; Jan Van Leusen; Paul Kögerler; Zheyuan Chen; John Bacsa; Yurii V. Geletii; Weiwei Guo; Tianquan Lian; Craig L. Hill

doi:10.1002/chem.201503010

^28-: A New Polyoxometalate Structural Family with Catalytic Hydrogen Evolution Activity

Hongjin Lv
, Yingnan Chi
, Jan Van Leusen
, Paul Kögerler
, Zheyuan Chen
, John Bacsa
, Yurii V. Geletii
, Weiwei Guo
, Tianquan Lian
, Craig L. Hill^*

^*Corresponding author for this work

Research output: Contribution to journal › Article › peer-review

55 Citations (Scopus)

Abstract

A new structural polyoxometalate motif, [{Ni₄(OH)₃AsO₄}₄(B-α-PW₉O₃₄)₄]^28-, which contains the highest nuclearity structurally characterized multi-nickel-containing polyanion to date, has been synthesized and characterized by single-crystal X-ray diffraction, temperature-dependent magnetism and several other techniques. The unique central {Ni₁₆(OH)₁₂O₄(AsO₄)₄} core shows dominant ferromagnetic exchange interactions, with maximum χ_mT of 69.21 cm³ K mol^-1 at 3.4 K. Significantly, this structurally unprecedented complex is an efficient, water-compatible, noble-metal-free catalyst for H₂ production upon visible light irradiation (photosensitizer=[Ir(ppy)₂(dtbbpy)][PF₆]; sacrificial electron donor=triethylamine or triethanolamine). The highest turnover number of approximately 580, corresponding to a best quantum yield of approximately 4.07 %, is achieved when using triethylamine as electron donor in the presence of water. The mechanism of this photodriven process has been probed by time-solved luminescence and by static emission quenching.

Original language	English
Pages (from-to)	17363-17370
Number of pages	8
Journal	Chemistry - A European Journal
Volume	21
Issue number	48
DOIs	https://doi.org/10.1002/chem.201503010
Publication status	Published - 23 Nov 2015
Externally published	Yes

Keywords

hydrogen production
nickel
photocatalysis
polyoxometalates
temperature-dependent magnetism

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Access to Document

10.1002/chem.201503010

Cite this

@article{13a52e86187b475499f5569567bb0dbb,

title = "28-: A New Polyoxometalate Structural Family with Catalytic Hydrogen Evolution Activity",

abstract = "A new structural polyoxometalate motif, [\{Ni4(OH)3AsO4\}4(B-α-PW9O34)4]28-, which contains the highest nuclearity structurally characterized multi-nickel-containing polyanion to date, has been synthesized and characterized by single-crystal X-ray diffraction, temperature-dependent magnetism and several other techniques. The unique central \{Ni16(OH)12O4(AsO4)4\} core shows dominant ferromagnetic exchange interactions, with maximum χmT of 69.21 cm3 K mol-1 at 3.4 K. Significantly, this structurally unprecedented complex is an efficient, water-compatible, noble-metal-free catalyst for H2 production upon visible light irradiation (photosensitizer=[Ir(ppy)2(dtbbpy)][PF6]; sacrificial electron donor=triethylamine or triethanolamine). The highest turnover number of approximately 580, corresponding to a best quantum yield of approximately 4.07 \%, is achieved when using triethylamine as electron donor in the presence of water. The mechanism of this photodriven process has been probed by time-solved luminescence and by static emission quenching.",

keywords = "hydrogen production, nickel, photocatalysis, polyoxometalates, temperature-dependent magnetism",

author = "Hongjin Lv and Yingnan Chi and \{Van Leusen\}, Jan and Paul K{\"o}gerler and Zheyuan Chen and John Bacsa and Geletii, \{Yurii V.\} and Weiwei Guo and Tianquan Lian and Hill, \{Craig L.\}",

note = "Publisher Copyright: {\textcopyright} 2015 WILEY-VCH Verlag GmbH \& Co. KGaA, Weinheim.",

year = "2015",

month = nov,

day = "23",

doi = "10.1002/chem.201503010",

language = "English",

volume = "21",

pages = "17363--17370",

journal = "Chemistry - A European Journal",

issn = "0947-6539",

publisher = "John Wiley and Sons Inc.",

number = "48",

}

TY - JOUR

T1 - 28-

T2 - A New Polyoxometalate Structural Family with Catalytic Hydrogen Evolution Activity

AU - Lv, Hongjin

AU - Chi, Yingnan

AU - Van Leusen, Jan

AU - Kögerler, Paul

AU - Chen, Zheyuan

AU - Bacsa, John

AU - Geletii, Yurii V.

AU - Guo, Weiwei

AU - Lian, Tianquan

AU - Hill, Craig L.

PY - 2015/11/23

Y1 - 2015/11/23

N2 - A new structural polyoxometalate motif, [{Ni4(OH)3AsO4}4(B-α-PW9O34)4]28-, which contains the highest nuclearity structurally characterized multi-nickel-containing polyanion to date, has been synthesized and characterized by single-crystal X-ray diffraction, temperature-dependent magnetism and several other techniques. The unique central {Ni16(OH)12O4(AsO4)4} core shows dominant ferromagnetic exchange interactions, with maximum χmT of 69.21 cm3 K mol-1 at 3.4 K. Significantly, this structurally unprecedented complex is an efficient, water-compatible, noble-metal-free catalyst for H2 production upon visible light irradiation (photosensitizer=[Ir(ppy)2(dtbbpy)][PF6]; sacrificial electron donor=triethylamine or triethanolamine). The highest turnover number of approximately 580, corresponding to a best quantum yield of approximately 4.07 %, is achieved when using triethylamine as electron donor in the presence of water. The mechanism of this photodriven process has been probed by time-solved luminescence and by static emission quenching.

AB - A new structural polyoxometalate motif, [{Ni4(OH)3AsO4}4(B-α-PW9O34)4]28-, which contains the highest nuclearity structurally characterized multi-nickel-containing polyanion to date, has been synthesized and characterized by single-crystal X-ray diffraction, temperature-dependent magnetism and several other techniques. The unique central {Ni16(OH)12O4(AsO4)4} core shows dominant ferromagnetic exchange interactions, with maximum χmT of 69.21 cm3 K mol-1 at 3.4 K. Significantly, this structurally unprecedented complex is an efficient, water-compatible, noble-metal-free catalyst for H2 production upon visible light irradiation (photosensitizer=[Ir(ppy)2(dtbbpy)][PF6]; sacrificial electron donor=triethylamine or triethanolamine). The highest turnover number of approximately 580, corresponding to a best quantum yield of approximately 4.07 %, is achieved when using triethylamine as electron donor in the presence of water. The mechanism of this photodriven process has been probed by time-solved luminescence and by static emission quenching.

KW - hydrogen production

KW - nickel

KW - photocatalysis

KW - polyoxometalates

KW - temperature-dependent magnetism

UR - https://www.scopus.com/pages/publications/84954349731

U2 - 10.1002/chem.201503010

DO - 10.1002/chem.201503010

M3 - Article

AN - SCOPUS:84954349731

SN - 0947-6539

VL - 21

SP - 17363

EP - 17370

JO - Chemistry - A European Journal

JF - Chemistry - A European Journal

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